CELLULOSE
·
2020
·Vol. 27
·期 17
·10167-10181
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IF 4.21
Guo Wanghuan,Zhao Zhigang,Yang Fan,Xie Meiying,Shao Zhiheng,Xue Liyan,Zhang Yang,Lin Wanqing,Du Chang,Zhang Yongjian
Abstract The separation and recovery of Au(III), Pd(II), and Pt(IV) is a challenge in hydrometallurgy, and finding good adsorbents is a way to solve this problem. In this work, two novel adsorbents, carboxymethyldiethylammoniumethyl cellulose (CM-n-DEAEC) and carboxymethyl-2-diethylaminoethyl cellulose (CM-o-DEAEC), were synthesized by changing the grafting site of carboxymethyl on diethylaminoethyl cellulose (DEAEC). The structures and morphologies of the adsorbents were examined by NMR, FT-IR, EA, TGA, and SEM analyses. The effects of adsorbents on the separation performance of Au(III), Pd(II), and Pt(IV) at different adsorption conditions were studied. The performances of stripping and recycling were investigated. At a 3 M chloride ion concentration, CM-n-DEAEC's adsorption rates for Pd(II), Au(III), and Pt(IV) were stabilized at 60%, 30%, and 7% in the pH range of 1.0–3.0 and were unaffected by coexisting metal ions. However, at a 0.1 M chloride ion concentration, CM-o-DEAEC separated Pt(IV) before Au(III) and Pd(II) in the pH range from 1.0 to 2.0 without being affected by coexisting metal ions. In addition, the absorbed metal ions can be easily stripped by a 0.1 M thiourea-0.1 M HCl solution, and the adsorption rate only decreased by 3.0% and 1.8% after seven adsorption–desorption cycles. Therefore, it was shown that CM-n-DEAEC and CM-o-DEAEC are excellent adsorbents that can control the adsorption order of precious metals and can selectively and quickly recover Pd(II) or Pt(IV) from wastes containing Au(III). Graphic abstract
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JOURNAL OF NON-CRYSTALLINE SOLIDS
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2020
·
IF 2.929
Shaoxia Wang,Meirong Shen,Jianfei Qu,Xuming Zhuang,Shou-Qing Ni,Xuran Wu
In this study, mercapto-modified graphene/multi-walled carbon nanotube aerogels were facilely constructed by using L-cysteine as a cross-linking agent and modifier. The effective adsorption behaviors of Au(III) from environmental samples by the aerogels were investigated. The aerogels were characterized, and many influencing factors, such as pH value, adsorbent dosage, and contact time, were optimized. The kinetic data followed the pseudo-second-order model, and the equilibrium data fitted well to the Freundlich isotherm model. The maximum adsorption capacity for Au(III) reached approximately 47 mg g −1 . Moreover, the Au(III) could be desorbed with 1 M HCl containing 4% thiourea and detected by inductively coupled plasma atomic emission spectroscopy. Finally, the aerogels were used in lake water, seawater, and soil samples for Au(III) adsorption with recovery rates from 87.0% to 102.8%. The results indicate that the developed aerogel is an excellent adsorbent for removing Au(III) from samples and has significant application prospects in environmental research.
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International Journal of Minerals Metallurgy and Materials
·
2026
·Vol. 33
·期 6
·1870-1885
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IF 8.8
He Baili,Kou Jue,Sun Chunbao,Li Yue,Li Xiaolin,Temirov Uktam,Chang Ziyong
The development of effective adsorbents is crucial for the sustainable recovery of noble metals from secondary resources. In this study, MIL-101(Cr)-Tu, a Cr-based metal–organic framework (MOF) modified with thiourea, was successfully prepared by double-phase encapsulation followed by post-synthetic modification. At 298 K, the largest adsorption capacities of Au(III), Pd(II), and Pt(IV) by MIL-101(Cr)-Tu were (1230.83 ± 8.72), (330.41 ± 7.29), and (315.58 ± 13.67) mg·g −1 , respectively. The uptakes of Au(III), Pd(II), and Pt(IV) increased with temperature. The adsorption data fit well to both the Langmuir and pseudo-second-order kinetic models, indicating that the adsorption process conformed to monolayer adsorption and chemisorption. Mechanistic analysis revealed that the amino and thiourea groups facilitated the adsorption of noble metals through coordination and electrostatic attraction. Notably, Au(III), Pd(II), and Pt(IV) interacted strongly with the thiourea groups owing to their “soft–soft” interactions. Moreover, Au(III) was reduced to Au(I) and Au(0), Pt(IV) was reduced to Pt(II), and the amino groups were oxidized to NO 2 . The adsorption of Pd(II) did not involve redox reactions. Additionally, MIL-101(Cr)-Tu exhibited strong selectivity for noble metals and excellent reusability, demonstrating its great potential for the extraction of noble metals from secondary resources.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Shuai Wang,Hao Wang,Shixing Wang,Libo Zhang,Likang Fu
The gold recovery from wastewater is not only beneficial to environmental protection, but also to alleviate the shortage of resources. Chitosan is considered as an excellent adsorption material, but its application in gold recovery is always some shortcomings including low adsorption capacity and selectivity. This work developed an efficient biosorbent (CS-ES) by functionalizing chitosan with poly(ethylene sulfide) for gold recovery from simulated wastewater. The properties and adsorption mechanism of CS-ES were investigated using SEM, EDS , XRD , FT-IR, BET and XPS . The results of experiments revealed that the adsorption efficiency of CS-ES for Au(III) reaches more than 90% in a wide pH range (2.0–6.0) and the highest adsorption efficiency about 99.07% was achieved at pH = 5.0. At 318 K, the highest adsorption ability of CS-ES for gold ions was 657.49 mg/g. The adsorption findings supported the Langmuir and pseudo-second-order models, suggesting that monolayer chemisorption is the dominant adsorption mechanism. The thermodynamic performance ( ΔH° and ΔS° > 0, ΔG° <0) showed that gold ion adsorption by CS-ES is spontaneous exothermic reaction. CS-ES shows an excellent reproducibility after four adsorption-desorption cycles and selectivity against six metal ions. Moreover, a variety of physicochemical and spectroscopic tests demonstrate the extremely effective adsorption and in-situ reduction of gold by CS-ES are based on electrostatic attraction, chelation, and reduction between gold and nitrogen/sulfur groups. In this work, a novel adsorbent for recovering Au(III) from wastewater was devised with great efficiency, selectivity and repeatability.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
·
IF 6.633
Yangyang Wang,Xiaoxia Liu,Annie Yang,Ping Lv,Lixin Zhang,Yongnian Li,Yanzhao Yang
Selective recovery of gold and platinum from secondary resources is of great significance under the crisis of resource shortage. Hence, the optimal extractant 1-(2-(dimethylamino) ethyl)-4-methyl-piperazin bis(trifluoromethylsulfonyl)imide ([C 6 -Et-TMEDA-PIP][Tf 2 N] 2 ) was synthesized and screened out from five piperazine-based ionic liquids (ILs) to construct an IL-water system for Au(III) and Pt(IV) extraction. ILs have high hydrophobicity and low viscosity at room temperature, which can be used as both extractant and hydrophobic phase. The effects of IL dosage, metal concentration and acidity on the extraction efficiency were investigated. Under the optimal conditions, the extraction efficiency of 98.5% (Au(III)) and 97.5% (Pt(IV)) can be achieved. The anion exchange mechanism was verified through the combination of Ultraviolet visible spectroscopy (UV–vis), Nuclear magnetic spectra (NMR) and quantum chemical calculations. Besides that, the two-factor optimization of the extractant dosage and HCl concentration was carried out by Response surface methodology (RSM), and the effective separation of Au(III) and Pt(IV) was successfully achieved. Au(III)/ Pt(IV) was extracted into the IL phase as [Et-TMEDA-PIP + ][AuCl 4 - ] and can easily be stripped by reduction to Au(0)/Pt(Ⅱ) with H 2 C 2 O 4 /CS(NH 2 ) 2 -HCl, and each extraction ability maintained after 5 turns of extraction cycle experiments. Since the excellent behaviors showed in the multi-metal selective extraction and cycle experiments, the [C 6 -Et-TMEDA-PIP][Tf 2 N] 2 was regarded as the most potential system for Au(III) and Pt(IV) recovery from HCI medium.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xuefeng Yu,Chuanhao Yan,Jinglei He,Jinlong Zhang,Hangzhou lv,Fuqiang Liu,Jianlong Wang,Junfeng Liu,Xilong Wang
To synthesize a novel magnetic nanomaterial for effective Au(III) recovery from the aqueous phase with excellent capability, superior selectivity, one-step reduction and ease of separation after loading Au(III) still remains a huge challenge. In this study, a magnetic nanomaterial (γ-Fe 2 O 3 @PDA-NAM) with a core–shell structure was synthesized for effective Au(III) recovery by sorption. The maximum Au(III) sorption capacity by γ-Fe 2 O 3 @PDA-NAM reached 2910 mg/g at pH = 6.10 ± 0.15, 44.29 times that by γ-Fe 2 O 3 (65.7 mg/g). Its Au(III) sorption efficiency was over 97.75% at very low concentrations (i.e., 5.5 × 10 -4 and 5.5 × 10 -5 mg/mL). TEM, XPS and FTIR analysis verified that excellent Au(III) recovery by γ-Fe 2 O 3 @PDA-NAM resulted from N/S-containing soft base moieties introduced to different layers. N and/or S elements at these sites provided lone pair electrons to Au(III) to form stable coordination bond. Meanwhile, the hydrogen bond between O-containing (–OH, -C=O) and N-containing (-C-N, -N(-C)-N-, -C=N) moieties on γ-Fe 2 O 3 @PDA-NAM and –OH on the main speciations of Au(III) (AuCl 3 (OH) - , AuCl 2 (OH) 2 - , and AuCl(OH) 3 - ) also greatly enhanced Au(III) recovery. About 78.03% of Au(III) was directly reduced to elemental gold by -C-S- and -N(-C)-N- group on the tertiary amine structure during sorption. More than 98.84% of Au(III) was selectively sorbed on γ-Fe 2 O 3 @PDA-NAM at pH 4.0 even though Pt(IV), Cu(II), Zn(II), Pb(II), and Ni(II) were co-present at the same concentration as that for Au(III) (0.01 mg/mL). In contrast, sorption efficiency of other interfering ions was within 1.75–26.05%. A relatively poor sorption selectivity for Pt(IV) could be acceptable because it is also a noble metal.
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Environmental Science-Nano
·
2023
·
IF 7.3
Chuanhao Yan,Xuefeng Yu,Jinlong Zhang,Jinglei He,Wenyi Jia,Jianlong Wang,Fuqiang Liu,Junfeng Liu,Xilong Wang
To significantly enhance the unsatisfactory Au(III) sorption performance (2280 mg g−1) by a material designed in our previous work, we ingeniously fabricated a nano-sized and uniform molybdenum composite (MoCOM) using a household microwave oven; it was embedded in a nanofiber mat by electrospinning technique to synthesize a novel material (CS-MoCOM-Th) for effective Au(III) sorption. After embedding MoCOM, an ultrahigh maximum sorption capacity (4090 mg g−1) of Au(III) at high concentrations and a sorption efficiency at low concentrations by CS-MoCOM-Th (99.59%) were achieved at pH 4.0. Mechanistically, the excellent Au(III) sorption performance was mainly driven by electrostatic attraction by protonated C–N+ groups and coordination interaction with N- or S-containing moieties: C–N, CN, C–N+, CS, S(−II), and Sn(−II). During sorption, 69.42% of Au(III) was directly reduced to elemental gold on CS-MoCOM-Th, and gold foils precipitated on the nanofiber mat. Notably, excellent sorption selectivity of Au(III) on CS-MoCOM-Th was achieved when heavy metals, including Cu(II), Ni(II), Pb(II), and Zn(II), and noble metal Pt(IV) were co-present at 2 × 10−3 mg mL−1. CS-MoCOM-Th could still sorb 82.15% of Au(III) at 0.01 mg mL−1 after four cycles. Overall, this study highlights that CS-MoCOM-Th is one of the most competitive candidates for Au(III) recovery from the aqueous phase.
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MICROCHEMICAL JOURNAL
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2020
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IF 3.594
Yu Hua,Jia-yuan Li,Hong Min,Xiao-hong Wu,Xiao-bing Cui,Yi-jun Chen,Hong-zhen Lian,Dong Sheng
In this work, by introducing solvothermal method for generating Fe 3 O 4 nanoparticles and “one-pot” method for synthesizing organic–inorganic hybrid monolithic vinyl functionalized Fe 3 O 4 (Fe 3 O 4 @HM), a facile procedure was proposed for preparing poly(1-vinylimidazole) (PVIM) functionalized gold ion imprinted polymer based MNPs@IIP (MNPs@HM@PVIM-Au-IIP). The as-prepared magnetic nanocomposites were characterized by scanning electron microscopy (SEM), transmission electron microscope (TEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and vibrating sample magnetometry (VSM), etc. After the optimum conditions, including solution pH, adsorption time and sample volume, eluent composition and volume, and elution time were investigated, this MNPs@IIP was employed as ion imprinted polymer magnetic solid phase extraction (II-MSPE) matrix for separation and enrichment of trace gold ions followed by inductively coupled plasma mass spectrometric (ICP-MS) determination with excellent selectivity and sensitivity, and strong anti-interference ability. These merits were benefited from the formation of hybrid monolithic interlayer enduing the resultant MNPs@HM@PVIM-Au-IIP with good chemical and mechanical stability, as well as the dimensional homogeneity due to the solvothermal-generated Fe 3 O 4 nanoparticles as the cores. The applicability superiority of this MNPs@IIP was confirmed by the rapid and efficient extraction of trace level Au(III) in environment water, sediment, soil, coal and ore samples with satisfactory results. The reliability of this II-MSPE-ICP-MS method was also verified by using corresponding Certified Standard Reference materials and spiking recovery of the real samples analyzed.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Fenglei Liu,Baowei Hu
Recovery of precious metal ions in wastewater could not only improve resource utilization, but also could reduce environmental pollution. Herein, a composite of TpPa@Nb 2 C was constructed by an interfacial self-assembled method and explored the synergistic adsorption effects for precious metals. The structure and morphology of the composites were analyzed by advanced characterization techniques, followed by parametric analysis of Au(III)/Pd(II) adsorption from the simulated wastewater. The results showed that the grafting of COFs with abundant reducing active sites on the MXenes could significantly improve the selectivity and adsorption capacity. Meanwhile, the interaction was found as monolayer way and controlled by chemistry process, and the maximum equilibrium Au(III) and Pd(II) uptake reached up to 910.1 and 386.2 mg/g, respectively. The competitive adsorption study showed that the co-existence of impurities had little effect on the removal rate. The mechanism analysis demonstrated that the precious metal ions were reduced to elemental gold/palladium on the network of TpPa@Nb 2 C, and they got three electrons or two electrons from the hydroxyl groups through redox reaction, respectively. Thus, this study provided an excellent material for enrichment and recovery of precious metals in waste liquid and the treatment of e-waste.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
·
IF 4
Zhiwei Wang,Guangyuan Hu,Changqing Xia,Xinliang Wang,Hongxing He,Zhifeng Nie,Shixing Wang,Weili Li
The recovery and utilization of precious metals from secondary resources are important owing to their pivotal role in modern technology. In this study, we successfully grafted diamine onto UiO-67, modulated its charge and functionalization, and developed a highly efficient adsorbent for the extraction of Au(III) from waste solutions. The recovery rate of UiO-67-(NH 2 ) 2 for trace gold is >99 % in the wide range of pH 3 to 9. The maximum adsorption capacity of UiO-67-(NH 2 ) 2 at a temperature of 298 K is 482 mg/L. In addition, UiO-67-(NH 2 ) 2 exhibits excellent selectivity to Au(III) in mixed metal ion waste solutions. After five cycles of adsorption–desorption experiments, the adsorption efficiency remains above 95 %. The identification of electrostatic interactions, coordination, and reduction as the primary adsorption mechanisms is supported by X-ray photoelectron spectroscopy (XPS) analysis of UiO-67-(NH 2 ) 2 and density functional theory (DFT) calculations.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 16
·7695-7703
·
IF 3.925
Qi Wu,Changfeng Zhao,Qinzhong Wang,Jing Liu
This study proposes the efficient separation of Au(III)/Pd(II)/Pt(IV)/Rh(III) through the 2-mercaptobenzothiazole-functionalised ionic liquid ([C6mim][2MBT]) using a cloud point extraction system. Direct cloud point extraction of Au(III) (about 99.9%) was realised without involving any functionalised ionic liquids. A significant enhancement of the Pd(II) extraction performance was found by adding rationally constructed [C6mim][2MBT]. Consequently, a fairly high extraction percentage of about 99.4% was obtained. However, further advancement of the proposed cloud point extraction showed that it could not be applied for the preconcentration of Pt(IV) and Rh(III) without adding stannous chloride, which plays a critical role in the segregation and could be adjusted by changing the hydrochloric acid concentration. Under the optimised conditions, the Rh(III) extraction process shows a high yield percentage (ca. 83.0%), where the majority of Pt(IV) was enriched in the aqueous phase. In addition, the underlying possible extraction mechanism was investigated using UV-vis, FT-IR and TEM measurements, which indicated that TX-114 acted as a solvent for the extracted metals. The developed procedure reveals efficient direct Au(III)/Pd(II)/Pt(IV)/Rh(III) separation using [C6mim][2MBT] via cloud point extraction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
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IF 9.1
Fei Chai,Haoran Chen,Hongrui Xiang,Feiping Zhao,Qingwei Wang,Xiaobo Min,Liyuan Chai
Selective separation of precious metals from chloride-rich acidic media remains challenging because of the complex aqueous speciation of metal ions and the interference of competing ions. In this study, a polyethyleneimine (PEI)-functionalized tannin-based phenolic resin (TPR@PEI), enriched with O/N binding sites, was synthesized via Schiff base reactions for the selective separation and recovery of Au(III) and Pd(II) from complex acidic chloride solutions. The effects of key synthesis parameters, including tannic acid (TA) dosage, formaldehyde (FA) volume and crosslinking time, on adsorbent structure and Au(III)/Pd(II) adsorption performance were systematically investigated. Under the optimized synthesis conditions (1 g TA, 5 mL FA, and 2 h crosslinking time), TPR@PEI exhibited rapid adsorption kinetics, reaching equilibrium within 40 min for both metal ions. The adsorption behavior was well described by the pseudo-second-order kinetic model and the Langmuir isotherm model, with maximum adsorption capacities of 416.67 mg g −1 for Au(III) and 270.27 mg g −1 for Pd(II) at pH 2. More importantly, TPR@PEI showed superior selectivity toward Au(III) (> 99%) and Pd(II) (> 87%) in both binary and multicomponent systems, and maintained removal efficiencies remaining above 90% over five adsorption-desorption cycles. Combined characterization and density functional theory calculations (DFT) revealed that the excellent separation performance was governed by the synergistic effects of electrostatic attraction, redox interaction, and coordination/chelation enabled by the cooperative O/N-rich binding sites. These results demonstrate that TPR@PEI is a promising adsorbent for the highly selective separation and recovery of precious metals from complex chloride-rich acidic solutions.
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